EP0178007A2 - Verfahren zur Erzeugung von Synthesegas - Google Patents

Verfahren zur Erzeugung von Synthesegas Download PDF

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Publication number
EP0178007A2
EP0178007A2 EP85201545A EP85201545A EP0178007A2 EP 0178007 A2 EP0178007 A2 EP 0178007A2 EP 85201545 A EP85201545 A EP 85201545A EP 85201545 A EP85201545 A EP 85201545A EP 0178007 A2 EP0178007 A2 EP 0178007A2
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EP
European Patent Office
Prior art keywords
stream
gaseous
synthesis gas
hydrocarbons
converted
Prior art date
Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
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Application number
EP85201545A
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English (en)
French (fr)
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EP0178007B1 (de
EP0178007A3 (en
Inventor
Jack Jacometti
Maarten Johannes Van Der Burgt
Johannes Didericus De Graaf
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Shell Internationale Research Maatschappij BV
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Shell Internationale Research Maatschappij BV
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Priority to AT85201545T priority Critical patent/ATE54120T1/de
Publication of EP0178007A2 publication Critical patent/EP0178007A2/de
Publication of EP0178007A3 publication Critical patent/EP0178007A3/en
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    • C—CHEMISTRY; METALLURGY
    • C07—ORGANIC CHEMISTRY
    • C07C—ACYCLIC OR CARBOCYCLIC COMPOUNDS
    • C07C1/00—Preparation of hydrocarbons from one or more compounds, none of them being a hydrocarbon
    • C07C1/02—Preparation of hydrocarbons from one or more compounds, none of them being a hydrocarbon from oxides of a carbon
    • C07C1/04—Preparation of hydrocarbons from one or more compounds, none of them being a hydrocarbon from oxides of a carbon from carbon monoxide with hydrogen
    • C07C1/0485—Set-up of reactors or accessories; Multi-step processes
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B3/00—Hydrogen; Gaseous mixtures containing hydrogen; Separation of hydrogen from mixtures containing it; Purification of hydrogen; Reversible storage of hydrogen
    • C01B3/02—Production of hydrogen; Production of gaseous mixtures containing hydrogen
    • C01B3/32—Production of hydrogen; Production of gaseous mixtures containing hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide or air
    • C01B3/34—Production of hydrogen; Production of gaseous mixtures containing hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide or air by reaction of hydrocarbons with gasifying agents
    • C01B3/36—Production of hydrogen; Production of gaseous mixtures containing hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide or air by reaction of hydrocarbons with gasifying agents using oxygen; using mixtures containing oxygen as gasifying agents

Definitions

  • the invention relates to a process for the production of synthesis gas with an increased H 2 /CO-ratio from normally gaseous hydrocarbons comprising the following steps:
  • An object of the invention is to increase the H 2 /CO-ratio of a synthesis gas resulting from the conversion of normally gaseous hydrocarbons thereby enabling the reaction of the carbon compuonds with an optimal or near optimal consumption of energy and materials in the manufacture of synthesis gas from gaseous fuels.
  • By-products and waste products from chemical synthesis and natural gas can be employed as the gaseous fuels.
  • the oxygen-containing gas may be pure oxygen, air or mixtures of pure oxygen and air.
  • the partial oxidation of gaseous feedstocks can take place according to various established processes.
  • the partial oxidation of gaseous fuels is usually carried out at temperatures around 900 to roughly 1600 °C, preferably 1100 to 1500 °C and pressures up to 100 bar, preferably 5 to 100 bar.
  • the resulting synthesis gas contains no ash, slag, soot or tar, thereby eliminating the necessity of using expensive purification steps.
  • Raised pressure, high temperature and a gaseous feed lead to a high degree of conversion and relative to the volume of the gasification chamber, they effect a high specific throughput.
  • synthesis gas converted into products such as ammonia, Oxo compounds, methanol or products from the Fischer-Tropsch synthesis and which operate under pressure
  • a considerable part of the investment required for the compression can be saved on partial oxidizing gaseous fuels under pressure.
  • the pressure partial oxidation of gaseous fuel permits a considerable saving in the manufacturing costs of synthesis gas.
  • Endothermic thermal or catalytic reaction of gaseous hydrocarbons, in the presence of steam to produce carbon monoxide and hydrogen is an established reaction which is operated industrially using various processes.
  • Such a process can be carried out in a tubular reactor, the necessary heat of reaction being supplied via heat transport through the walls of the tubes or in a medium of externally heated solid heat exchanger material e.g. fine grained solid which is used in a fluidized bed.
  • the gaseous mixture comprising H 2 and CO formed in the conversion of normally gaseous hydrocarbon(s) with steam (step b) is separated into a Co-containing stream and an H 2 stream.
  • This separation step (c) can be carried out in every possible way e.g. cryogenicly, by means of membranes, adsorption and/or adsorption.
  • the co-containing stream resulting from separation step (c) mainly consists of CO, CO 2 and CH 4 . At least part of it is preferably used for burning and at least part of the heat generated in this way is used for the conversion of the normally gaseous hydrocarbons in step (b).
  • At least part of the substantially pure hydrogen stream separated in step (c) is mixed with the synthesis gas produced in step (a).
  • the H 2 /CO-ratio of this gas is preferably increased to a value in the range from 1.8 t 2.5.
  • Such as gas is very suitable for the synthesis of hydrocarbons according to the Fischer-Tropsch process, which process is described in the book "The Fischer-Tropsch and Related Syntheses" by H.H. Storch, N. Golumbic and R.B. Anderson (1951). Therefore the gas obtained in step (d) is at least in part catalytically converted in to a product comprising a hydrocarbon mixture.
  • the invention also relates to a process for the production of a hydrocarbon mixture by the catalytic conversion of the synthesis gas produced in step (d) of the present synthesis gas generating process.
  • the product comprising a hydrocarban mixture is preferably separated into a gaseous stream comprising non-converted CO and H 2 and low-boiling hydrocarbons, and at least one stream comprising normally liquid hydrocarbons.
  • This separation can be carried out in any possible manner.
  • Advantageously fractional distillation is used for this purpose.
  • the low-boiling hydrocarbons present in the gaseous stream also comprising CO and H 2' suitably consist of C 1 -C 4 - hydrocarbons, but higher boiling hydrocarbons may be present in this stream too.
  • At least part of the gaseous stream comprising CO and H 2 and low-boiling hydrocarbons is preferably burned, suitably in a furnace, and at least part the heat generated by this burning is used for the endothermic conversion of at least part of the normally gaseous hydrocarbons with steam in step (b) of the present synthesis gas generating process.
  • At least part of the gaseous stream comprising CO and H 2 and low-boiling hydrocarbons is used as at least a part of the feed to step (b) in order to be converted with steam into the gaseous mixture comprising H 2 and CO.
  • At least part of the gaseous stream comprising CO and H 2 and low-boiling hydrocarbons is recycled to step (a) to be partially oxidized to synthesis gas.
  • At least one stream comprising normally liquid hydrocarbons is preferably separated from the product comprising a hydrocarbon mixture.
  • At least part of this (these) normally liquid hydrocarbons-containing stream(s) is (are) catalytically hydrocracked, advantageously using at least part of the H 2 stream separated in step (c) of the present process.
  • This hydrocracking step can be carried out in any possible way known in the art. Preference is given to a hydrocracking process using a supported noble metal catalyst as described in European patent application No. 84,201,256.9.
  • the product of the hydrocracking step is preferably subjected to a fractional distillation, at least one normally gaseous fraction comprising non-converted hydrogen and low-boiling hydrocarbons, at least one naphtha fraction, at least one kerosene fraction and at least one gas oil fraction being separated from the hydrocracking product.
  • the naphtha, kerosene and gasoil fractions are withdrawn fran the present process as final products.
  • the normally gaseous fraction(s) comprising non-converted hydrogen and low-boiling hydrocarbons is (are) preferably recycled as a feed to step (a) and/or step (b) of the present process and/or is (are) advantageously burned for generating heat which is at least in part used in step (b) of the present synthesis gas production process.
  • the synthesis gas with increased H 2/ CO-ratio which is produced in step (d) of the present synthesis gas production process can not only be used for the production of hydrocarbons but also as a feedstock for methanol production.
  • step (d) is advantageously converted into a product comprising methanol.
  • a gaseous stream comprising non-converted CO and H 2 is separated from this product and at least part thereof is burned for generating heat which is at least in part used for the conversion of at least part of the gaseous hydrocarbons with steam in step (b) of the present synthesis gas production process.
  • Substantially pure methanol is separated from the product of the methanol synthesis step and withdrawn as the final product of this step, while heavier products than methanol being obtained in this separation step are advantageously recycled to steps (a) or (b) of the present process to be used as feedstock for these steps and/or as a means for generating heat for step (b).
  • Natural gas is introduced via a line 1 into a desulphuri- zation unit 2 where sulphur compounds (H 2 S) are removed therefrom.
  • the desulphurized natural gas stream is passed via a line 3 into a gasification unit 4 where it is converted by partial oxidation into synthesis gas, mainly consisting of CO and H 2 .
  • air is introduced via a line 5 into an air separation unit 6 where it is separated into a N 2 -cootaining stream, withdrawn via a line 7 and a substantially pure oxygen stream passed via a line 8 to a line 9 where it is mixed with steam introduced into the system via a line 10.
  • the oxygen/steam mixture is passed via the line 9 into the gasification unit 4 where it is reacted with the desulphurized natural gas.
  • the resulting synthesis gas having an H 2 /CO-ratio below 1.7 is withdrawn from the gasifier 4 via a line 11. It is mixed with substantially pure hydrogen introduced via a line 12 and the mixture having an H 2 /CO-ratio in the range from 1.8 to 2.5 is passed via a line 13 to a hydrocarbon synthesis unit 14 where it is at least in part converted to hydrocarbons.
  • Non-converted H 2 and CO-containing gas mixture together with low boiling hydrocarbons (C1-C4) is withdrawn from the unit 14 via a line 15.
  • Part of this gas mixture is introduced via a line 16 into a steam reforming unit 17 where it is converted with steam (not shown) into an H 2 and CO-containing gas mixture having a higher H 2 /CO-ratio than the synthesis gas produced in the gasifier 4.
  • Part of the gas mixture withdrawn from the unit 14 via the line 15 is mixed with a CO-containing stream introduced via a line 18 into a line 19 and the mixture is passed via the line 19 to the burners (not shown) of the steam reforming unit 17 where the mixture is burned in order to furnish the heat for the endothermic steam reforming reactions.
  • the synthesis gas produced in unit 17 is passed to a pressure swing adsorber 20 in which it is separated into a CO-containing stream withdrawn via the line 18 and a H2-strearn withdrawn via a line 21.
  • Part of the H 2- stream is passed via the line 12 to the line 13.
  • An other part of the H 2- stream is passed via a line 22 to a hydrocracking unit 23 where it is used for hydrocracking normally liquid hydrocarbons produced in the synthesis unit 14 and passed from unit 14 to unit 23 through a line 24.
  • the hydrocracking product is passed from the hydrocracking unit 23 via a line 25 to a fractional distillation unit 26 where it is separated into a normally gaseous stream containing non-converted H 2 and light hydrocarbons, a naphtha stream, a kerosene stream and a gasoil stream, which streams are withdrawn from the system via lines 27, 28, 29 and 30 respectively.

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  • Chemical & Material Sciences (AREA)
  • Organic Chemistry (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Engineering & Computer Science (AREA)
  • General Chemical & Material Sciences (AREA)
  • Combustion & Propulsion (AREA)
  • Inorganic Chemistry (AREA)
  • General Health & Medical Sciences (AREA)
  • Health & Medical Sciences (AREA)
  • Oil, Petroleum & Natural Gas (AREA)
  • Hydrogen, Water And Hydrids (AREA)
  • Organic Low-Molecular-Weight Compounds And Preparation Thereof (AREA)
  • Catalysts (AREA)
  • Carbon And Carbon Compounds (AREA)
  • Electrolytic Production Of Non-Metals, Compounds, Apparatuses Therefor (AREA)
  • Glass Compositions (AREA)
EP85201545A 1984-10-10 1985-09-25 Verfahren zur Erzeugung von Synthesegas Expired - Lifetime EP0178007B1 (de)

Priority Applications (1)

Application Number Priority Date Filing Date Title
AT85201545T ATE54120T1 (de) 1984-10-10 1985-09-25 Verfahren zur erzeugung von synthesegas.

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
GB8425620 1984-10-10
GB08425620A GB2165551B (en) 1984-10-10 1984-10-10 Process for the production of synthesis gas

Publications (3)

Publication Number Publication Date
EP0178007A2 true EP0178007A2 (de) 1986-04-16
EP0178007A3 EP0178007A3 (en) 1987-08-12
EP0178007B1 EP0178007B1 (de) 1990-06-27

Family

ID=10567988

Family Applications (1)

Application Number Title Priority Date Filing Date
EP85201545A Expired - Lifetime EP0178007B1 (de) 1984-10-10 1985-09-25 Verfahren zur Erzeugung von Synthesegas

Country Status (13)

Country Link
EP (1) EP0178007B1 (de)
JP (1) JPH07100796B2 (de)
CN (1) CN1003580B (de)
AT (1) ATE54120T1 (de)
AU (1) AU570134B2 (de)
BR (1) BR8504974A (de)
CA (1) CA1292619C (de)
DE (1) DE3578411D1 (de)
ES (1) ES8604831A1 (de)
GB (1) GB2165551B (de)
IN (1) IN165968B (de)
NZ (1) NZ213732A (de)
ZA (1) ZA857734B (de)

Cited By (10)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
DE3803080A1 (de) * 1988-02-03 1989-08-17 Uhde Gmbh Verfahren zur erzeugung von synthesegasen aus kohlenwasserstoffhaltigen einsatzstoffen
FR2789691A1 (fr) * 1999-02-11 2000-08-18 Inst Francais Du Petrole Procede de synthese de distillat atmospherique comprenant l'utilisation de la technologie fischer-tropsch
WO2000068339A1 (en) * 1999-05-07 2000-11-16 Rentech, Inc. Convertible methanol/fischer-tropsch plant and method
EP0989093A3 (de) * 1998-09-21 2000-11-22 Air Products And Chemicals, Inc. Synthesegasherstellung mittels leitender Mischmembranen mit integrierter Konvertierung zu flüssigen Produkten
WO2001010979A1 (en) * 1999-08-05 2001-02-15 Atlantic Richfield Company Integrated process for converting hydrocarbon gas to liquids
US6479557B1 (en) 1999-02-15 2002-11-12 Shell Oil Company Process for the preparation of hydrocarbons from carbon monoxide and hydrogen
US6743829B2 (en) 2002-01-18 2004-06-01 Bp Corporation North America Inc. Integrated processing of natural gas into liquid products
EP1746143A1 (de) * 2005-07-20 2007-01-24 Shell Internationale Research Maatschappij B.V. Fischer-Tropsch Verfahren
WO2007009952A1 (en) * 2005-07-20 2007-01-25 Shell Internationale Research Maatschappij B.V. Multi stage fischer-tropsch process
US7168265B2 (en) 2003-03-27 2007-01-30 Bp Corporation North America Inc. Integrated processing of natural gas into liquid products

Families Citing this family (8)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
EP0191522B2 (de) * 1985-02-13 1996-12-18 Shell Internationale Researchmaatschappij B.V. Verfahren zur Erzeugung eines Wasserstoff enthaltenden Gases aus Kohlenwasserstoffen, Wasserdampf und/ggf. Kohlendioxid
GB2237814A (en) * 1989-11-10 1991-05-15 Shell Int Research A method and apparatus for co-generating power and hydrocarbons from coal derived synthesis gas using pressure swing absorption
RU2158711C1 (ru) * 2000-04-17 2000-11-10 Пискунов Семен Евсеевич Способ получения синтез-газа
US20100256246A1 (en) * 2009-04-06 2010-10-07 Rentech, Inc. System and method for conditioning biomass-derived synthesis gas
US20120291351A1 (en) * 2011-05-16 2012-11-22 Lawrence Bool Reforming methane and higher hydrocarbons in syngas streams
CA2851739C (en) 2011-10-18 2019-06-11 Shell Internationale Research Maatschappij B.V. Production of synthesis gas
RU2555043C1 (ru) * 2013-09-11 2015-07-10 Общество с ограниченной ответственностью "Газохим Техно" Способ очистки воды, образующейся на стадии синтеза углеводородов в процессе gtl, и способ ее использования
EP3599218A1 (de) * 2015-10-01 2020-01-29 L'air Liquide, Société Anonyme Pour L'Étude Et L'exploitation Des Procédés Georges Claude Verfahren und anlage zur erzeugung von synthesegas mit variabler zusammensetzung

Citations (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US3699218A (en) 1970-06-12 1972-10-17 Chevron Res Hydrogen manufacture

Family Cites Families (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
GB1458666A (en) * 1973-03-19 1976-12-15 Shell Internationel Mij Bv Process for the preparation of a methane-rich gas
US4110359A (en) * 1976-12-10 1978-08-29 Texaco Development Corporation Production of cleaned and purified synthesis gas and carbon monoxide
AR216940A1 (es) * 1977-06-28 1980-02-15 Texaco Development Corp Procedimiento para la produccion simultanea de una corriente de producto de gas de sintesis purificado y una corriente de producto de gas rico en co
CA1240708A (en) * 1983-11-15 1988-08-16 Johannes K. Minderhoud Process for the preparation of hydrocarbons

Patent Citations (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US3699218A (en) 1970-06-12 1972-10-17 Chevron Res Hydrogen manufacture

Non-Patent Citations (3)

* Cited by examiner, † Cited by third party
Title
H.H. STORCH, N. GOLUMBIC, R.B. ANDERSON: "The Fischer-Tropsch and Related Syntheses", 1951
KIRK-OTHMER: "Encyclopedia of chemical technology", vol. 21, 1980, pages: 543
OIL AND GAS JOURNAL, 6 September 1971 (1971-09-06), pages 85 - 90

Cited By (13)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
DE3803080A1 (de) * 1988-02-03 1989-08-17 Uhde Gmbh Verfahren zur erzeugung von synthesegasen aus kohlenwasserstoffhaltigen einsatzstoffen
EP0989093A3 (de) * 1998-09-21 2000-11-22 Air Products And Chemicals, Inc. Synthesegasherstellung mittels leitender Mischmembranen mit integrierter Konvertierung zu flüssigen Produkten
US6310108B1 (en) 1999-02-11 2001-10-30 Institut Francais Du Petrole Process for synthesis at atmospheric distillate that comprises the use of Fischer-Tropsch technology
FR2789691A1 (fr) * 1999-02-11 2000-08-18 Inst Francais Du Petrole Procede de synthese de distillat atmospherique comprenant l'utilisation de la technologie fischer-tropsch
US6479557B1 (en) 1999-02-15 2002-11-12 Shell Oil Company Process for the preparation of hydrocarbons from carbon monoxide and hydrogen
WO2000068339A1 (en) * 1999-05-07 2000-11-16 Rentech, Inc. Convertible methanol/fischer-tropsch plant and method
WO2001010979A1 (en) * 1999-08-05 2001-02-15 Atlantic Richfield Company Integrated process for converting hydrocarbon gas to liquids
AU774815B2 (en) * 1999-08-05 2004-07-08 Atlantic Richfield Company Integrated process for converting hydrocarbon gas to liquids
US6743829B2 (en) 2002-01-18 2004-06-01 Bp Corporation North America Inc. Integrated processing of natural gas into liquid products
US7168265B2 (en) 2003-03-27 2007-01-30 Bp Corporation North America Inc. Integrated processing of natural gas into liquid products
EP1746143A1 (de) * 2005-07-20 2007-01-24 Shell Internationale Research Maatschappij B.V. Fischer-Tropsch Verfahren
WO2007009952A1 (en) * 2005-07-20 2007-01-25 Shell Internationale Research Maatschappij B.V. Multi stage fischer-tropsch process
US7795318B2 (en) 2005-07-20 2010-09-14 Shell Oil Company Multi stage Fischer-Tropsch process

Also Published As

Publication number Publication date
EP0178007B1 (de) 1990-06-27
AU570134B2 (en) 1988-03-03
CA1292619C (en) 1991-12-03
NZ213732A (en) 1989-03-29
JPH07100796B2 (ja) 1995-11-01
GB2165551B (en) 1988-08-17
ZA857734B (en) 1986-05-28
ATE54120T1 (de) 1990-07-15
AU4836985A (en) 1986-04-17
ES547666A0 (es) 1986-03-01
CN85107305A (zh) 1986-07-09
GB8425620D0 (en) 1984-11-14
DE3578411D1 (de) 1990-08-02
EP0178007A3 (en) 1987-08-12
JPS6191292A (ja) 1986-05-09
BR8504974A (pt) 1986-07-22
ES8604831A1 (es) 1986-03-01
IN165968B (de) 1990-02-17
GB2165551A (en) 1986-04-16
CN1003580B (zh) 1989-03-15

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